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Hall was born Shirley Grossman in Philadelphia, Pennsylvania in 1922,[4] the only child of Eleanor and Joseph Grossman. Her father was from Latvia and her mother, who had acted in the Yiddish theatre, was from South Africa. Both were from Jewish immigrant families.[2]

When Hall was eight, her parents separated but never divorced. Hall became interested in acting, as an escape from a painful childhood, and auditioned for plays in New York City while she was still attending Simon Gratz High School. She enrolled at Temple University but did not matriculate. She landed her first professional job doing summer stock in Long Island in 1942.

In 1946, she married fellow actor Bradbart "Ted" Brooks in Los Angeles, California. They separated in 1949 and she returned to New York. In 1952, she married writer Sam Hall. Their son, Matthew, was born in 1958. She had always used the stage name Shirley Grayson, but Sam Hall called her Grayson, "like an old Army buddy", she said in an interview. She eventually adopted Grayson Hall as her professional name.[2]

Having guest starred on various television programs during the mid-1950s, Hall made her film debut in 1961 in Run Across the River. Hall also made Satan in High Heels, starring Meg Myles, in which Hall portrayed a cabaret club owner named Pepe. She later disavowed the film.

She was nominated for an Academy Award in the category of Best Supporting Actress for her performance as Judith Fellowes, a latent lesbian women's college instructor. In the original play, the character was not sympathetic but Huston rewrote the character, wanting more complexity and sympathy. She was featured as a kidnapped bank teller in Walt Disney's That Darn Cat! in 1965. In 1967, she played a high-profile middle-aged literary editor who becomes a Thrush agent on the television series The Man from U.N.C.L.E., in an episode written by Harlan Ellison.[6]

Hall's best-known television role was that of Dr. Julia Hoffman, on Dark Shadows, where she portrayed the loyal confidant and friend of the vampire, Barnabas Collins (Jonathan Frid). Other key roles that she played on the show were those of Countess Natalie Dupres; Magda Rakosi, a Gypsy; Hoffman, a Mrs. Danvers-type housekeeper, Julia Collins; and Constance Collins, sister of Brutus Collins.[7] She also appeared in both "Dark Shadows" feature films: House of Dark Shadows, again as Dr. Julia Hoffman, and Night of Dark Shadows, as a new character, housekeeper Carlotta Drake.[6]

Before appearing in The Night of the Iguana and Dark Shadows, Hall had an active stage career in New York City. She portrayed Irma, the madam of a most irregular bordello in the midst of a revolutionary uprising in Jean Genet's play The Balcony for more than a year at the Circle in the Square theatre in Greenwich Village. It was the longest running off-Broadway play for many decades. She was succeeded in the role by Nancy Marchand.[8]